Postsynthetically Tailoring Acid Properties and Pore Structures of ZnZrOx/MFI Catalysts for One-Pass CO2 Hydrogenation

IF 4.3 Q2 ENGINEERING, CHEMICAL

ACS Engineering Au Pub Date : 2023-09-21 DOI:10.1021/acsengineeringau.3c00027

Duanxing Li, Xiaofei Lu, Hiroka Kinoshita, Masanori Takemoto, Anand Chokkalingam, Shohei Tada* and Kenta Iyoki*,

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Abstract

This study investigated the performance of tandem catalysts, comprising a physical mixture of ZnZrO_x and MFI-type zeolites, in one-pass CO₂ hydrogenation. To finely adjust both the acidic properties and the pore structures, an alkali treatment was applied to a commercial zeolite. The alkali treatment resulted in enhanced catalytic activity and increased yields of C_2–4 olefin, C_2–4 paraffin, and C₅₊ hydrocarbon products, meanwhile suppressing coke formation and increasing the olefin to paraffin ratios. Comprehensive characterizations revealed that the development of the mesopore structure contributed to the observed enhancements in activity and hydrocarbon yields, with the decreased acid number rationalizing the increase in olefin to paraffin ratios. Reduced coke formation was attributed to both mesopore formation and increased external surfaces and optimized acid properties..

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ZnZrOx/MFI一次加氢催化剂的酸性质和孔结构

本研究研究了包括ZnZrOx和MFI型沸石的物理混合物的串联催化剂在单程CO2加氢中的性能。为了精细地调节酸性性质和孔结构，对商业沸石进行碱处理。碱处理提高了催化活性，提高了C2–4烯烃、C2–4链烷烃和C5+烃产物的产率，同时抑制了焦炭的形成，提高了烯烃与链烷烃的比例。综合表征表明，中孔结构的发展有助于观察到的活性和烃产率的提高，酸值的降低使烯烃与链烷烃比率的增加合理化。焦炭形成的减少归因于中孔的形成、外表面的增加和酸性质的优化。。

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ACS Engineering Au 化学工程技术-

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期刊介绍：）ACS Engineering Au is an open access journal that reports significant advances in chemical engineering applied chemistry and energy covering fundamentals processes and products. The journal's broad scope includes experimental theoretical mathematical computational chemical and physical research from academic and industrial settings. Short letters comprehensive articles reviews and perspectives are welcome on topics that include:Fundamental research in such areas as thermodynamics transport phenomena (flow mixing mass & heat transfer) chemical reaction kinetics and engineering catalysis separations interfacial phenomena and materialsProcess design development and intensification (e.g. process technologies for chemicals and materials synthesis and design methods process intensification multiphase reactors scale-up systems analysis process control data correlation schemes modeling machine learning Artificial Intelligence)Product research and development involving chemical and engineering aspects (e.g. catalysts plastics elastomers fibers adhesives coatings paper membranes lubricants ceramics aerosols fluidic devices intensified process equipment)Energy and fuels (e.g. pre-treatment processing and utilization of renewable energy resources; processing and utilization of fuels; properties and structure or molecular composition of both raw fuels and refined products; fuel cells hydrogen batteries; photochemical fuel and energy production; decarbonization; electrification; microwave; cavitation)Measurement techniques computational models and data on thermo-physical thermodynamic and transport properties of materials and phase equilibrium behaviorNew methods models and tools (e.g. real-time data analytics multi-scale models physics informed machine learning models machine learning enhanced physics-based models soft sensors high-performance computing)